Alternant Hydrocarbon Diradicals as Optically Addressable Molecular Qubits

• URL: http://arxiv.org/abs/2403.09102v2
• Date: Mon, 18 Mar 2024 00:53:05 GMT
• Title: Alternant Hydrocarbon Diradicals as Optically Addressable Molecular Qubits
• Authors: Yong Rui Poh, Dmitry Morozov, Nathanael P. Kazmierczak, Ryan G. Hadt, Gerrit Groenhof, Joel Yuen-Zhou,
• Abstract summary: High-spin molecules allow for bottom-up qubit design and are promising platforms for magnetic sensing and quantum information science. We use alternancy symmetry to selectively minimise radical-radical interactions in the ground state, generating $pi$-systems with high diradical characters.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: High-spin molecules allow for bottom-up qubit design and are promising platforms for magnetic sensing and quantum information science. Optical addressability of molecular electron spins has also been proposed in first-row transition metal complexes via optically-detected magnetic resonance (ODMR) mechanisms analogous to the diamond-NV colour centre. However, significantly less progress has been made on the front of metal-free molecules, which can deliver lower costs and milder environmental impacts. At present, most luminescent open-shell organic molecules are $\pi$-diradicals, but such systems often suffer from poor ground-state open-shell characters necessary to realise a stable ground-state molecular qubit. In this work, we use alternancy symmetry to selectively minimise radical-radical interactions in the ground state, generating $\pi$-systems with high diradical characters. We call them m-dimers, referencing the need to covalently link two benzylic radicals at their meta carbon atoms for the desired symmetry. Through a detailed electronic structure analysis, we find that the excited states of alternant hydrocarbon m-diradicals contain important symmetries that can be used to construct ODMR mechanisms leading to ground-state spin polarisation. The molecular parameters are set in the context of a tris(2,4,6-trichlorophenyl)methyl (TTM) radical dimer covalently tethered at the meta position, demonstrating the feasibility of alternant m-diradicals as molecular colour centres.

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